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Stable Cu/Cu2O/CuN3@NC Catalysts for Aqueous Phase Reforming of Methanol

Minglei Lu,Zhuoyu Zheng,Weiwei Lu,Haiping Zhu,Junwei Liao,Yuxin Ge,Xueer Huang,Qian Zhang,Jiajin Li,Yiyuan Zhou,Xiaoping Wu,Baozhu Chen,Chunxiao Yang,Xitang Qian,Minhua Shao,Tiejun Wang

Aqueous-phase reforming of methanol represents a promising avenue for hydrogen (H2) production. However, developing highly efficient and low-cost nonprecious catalysts remains challenging. Here, we report the synthesis of Cu-based catalysts with Cu, Cu2O, and CuN3 nanoparticles anchored on the nitrogen-doped carbon, forming Cu0/Cu+/Cu-N3 active sites. This catalyst achieves a H2 production rate of 140.1 μmol/gcat/s at 210 °C, which is several times to 2 orders of magnitude higher than that of Cu-, Ni-, even Pt-based catalysts, demonstrating excellent long-term stability over 350 h at 210 °C. A mechanism investigation reveals that the Cu-N3 site facilitates water dissociation into *OH and improves *CO and *OH conversion, leading to enhanced CO conversion and H2 production kinetics.